Chengye Song, Yan Zhao, Zonghao Liu, Yueqing Zhang, Jiahao Lai, Chaoqun Tan, Min Song
Low-temperature plasma, generating both reductive electrons and diverse oxidative species, has demonstrated considerable potential for the degradation of perfluorooctanoic acid (PFOA). However, limited understanding of electron propagation mechanisms during discharge has led previous research to focus on hydrated electrons (eaq–) while neglecting free electrons (e–). In this study, a consistent and modeled dielectric barrier discharge (DBD) plasma was employed to degrade PFOA. Contribution analysis indicated that reactions driven by e– were dominant, with substantial contributions from hydroxyl radical (•OH)-mediated oxidation. By integrating a kinetic model with a streamer solver, a basic discharge unit model was developed. Simulation of e– streamer propagation identified a high-intensity response electric field formed by the e– memory effect, with a peak strength of 1.816 × 106 V/m. This electric field facilitated a secondary acceleration of e–, allowing e– to penetrate the surface water layer and directly attack PFOA via chain-shortening mechanisms. The delocalized state of e– restricted degradation primarily to the gas–liquid interface, minimizing interference from the surrounding medium. This study highlights the previously overlooked role of e– and provides essential theoretical insights for the plasma-based treatment of PFOA-contaminated water.
{"title":"Plasma-Generated Free Electrons Induced Perfluorooctanoic Acid Efficient Degradation at the Gas–Liquid Interface","authors":"Chengye Song, Yan Zhao, Zonghao Liu, Yueqing Zhang, Jiahao Lai, Chaoqun Tan, Min Song","doi":"10.1021/acs.est.5c02062","DOIUrl":"https://doi.org/10.1021/acs.est.5c02062","url":null,"abstract":"Low-temperature plasma, generating both reductive electrons and diverse oxidative species, has demonstrated considerable potential for the degradation of perfluorooctanoic acid (PFOA). However, limited understanding of electron propagation mechanisms during discharge has led previous research to focus on hydrated electrons (e<sub>aq</sub><sup>–</sup>) while neglecting free electrons (e<sup>–</sup>). In this study, a consistent and modeled dielectric barrier discharge (DBD) plasma was employed to degrade PFOA. Contribution analysis indicated that reactions driven by e<sup>–</sup> were dominant, with substantial contributions from hydroxyl radical (•OH)-mediated oxidation. By integrating a kinetic model with a streamer solver, a basic discharge unit model was developed. Simulation of e<sup>–</sup> streamer propagation identified a high-intensity response electric field formed by the e<sup>–</sup> memory effect, with a peak strength of 1.816 × 10<sup>6</sup> V/m. This electric field facilitated a secondary acceleration of e<sup>–</sup>, allowing e<sup>–</sup> to penetrate the surface water layer and directly attack PFOA via chain-shortening mechanisms. The delocalized state of e<sup>–</sup> restricted degradation primarily to the gas–liquid interface, minimizing interference from the surrounding medium. This study highlights the previously overlooked role of e<sup>–</sup> and provides essential theoretical insights for the plasma-based treatment of PFOA-contaminated water.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"67 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758129","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Qi Wang, Yuefei Ruan, Yetong Shao, Linjie Jin, Naiyu Xie, Xiaoqiang Yang, Yuanyuan Hong, He Wang, Akira Tsujimoto, Moriaki Yasuhara, Kenneth Mei Yee Leung, Paul K. S. Lam
Per- and polyfluoroalkyl substances (PFAS) are synthetic long-lasting chemicals. Marine sediment is a major repository for PFAS in the environment; accordingly, this work investigated 45 legacy and emerging PFAS in samples of surface sediments and sediment cores (1940s–2020s) collected in the Pearl River outlets, its estuary, and the adjacent northern South China Sea (NSCS), one of the global pollution hotspots. The range of total PFAS concentrations in surface sediments from the river outlets and the NSCS was 244–14400 pg/g dry weight (dw) and 31.6–363 pg/g dw, respectively. In sediment cores, perfluorooctanesulfonate (PFOS) concentrations initially increased and then declined around ten years ago. Levels of long-chain perfluorinated carboxylates have been increasing since the 1980s and experienced an accelerated rise in the 2000s. Hydrogen-substituted polyfluoroalkyl ether sulfonate (H-PFESA) was widely found in sediment samples for the first time. The ratios of 6:2 H-PFESA to 6:2 chlorinated (Cl-) PFESA in sediment cores exceeded those in surface sediment and exhibited an increasing trend with the sediment age, implying the gradual transformation of 6:2 Cl-PFESA to its hydrogen-substituted analog in sediments. A preliminary risk assessment indicated that ∑6:2 PFESAs and PFOS posed medium to high risks over recent decades.
{"title":"Spatiotemporal Trend of PFAS in Estuarine Sediments: Insights into Chlorinated Polyfluoroalkyl Ether Sulfonate Transformation","authors":"Qi Wang, Yuefei Ruan, Yetong Shao, Linjie Jin, Naiyu Xie, Xiaoqiang Yang, Yuanyuan Hong, He Wang, Akira Tsujimoto, Moriaki Yasuhara, Kenneth Mei Yee Leung, Paul K. S. Lam","doi":"10.1021/acs.est.5c02731","DOIUrl":"https://doi.org/10.1021/acs.est.5c02731","url":null,"abstract":"Per- and polyfluoroalkyl substances (PFAS) are synthetic long-lasting chemicals. Marine sediment is a major repository for PFAS in the environment; accordingly, this work investigated 45 legacy and emerging PFAS in samples of surface sediments and sediment cores (1940s–2020s) collected in the Pearl River outlets, its estuary, and the adjacent northern South China Sea (NSCS), one of the global pollution hotspots. The range of total PFAS concentrations in surface sediments from the river outlets and the NSCS was 244–14400 pg/g dry weight (dw) and 31.6–363 pg/g dw, respectively. In sediment cores, perfluorooctanesulfonate (PFOS) concentrations initially increased and then declined around ten years ago. Levels of long-chain perfluorinated carboxylates have been increasing since the 1980s and experienced an accelerated rise in the 2000s. Hydrogen-substituted polyfluoroalkyl ether sulfonate (H-PFESA) was widely found in sediment samples for the first time. The ratios of 6:2 H-PFESA to 6:2 chlorinated (Cl-) PFESA in sediment cores exceeded those in surface sediment and exhibited an increasing trend with the sediment age, implying the gradual transformation of 6:2 Cl-PFESA to its hydrogen-substituted analog in sediments. A preliminary risk assessment indicated that ∑6:2 PFESAs and PFOS posed medium to high risks over recent decades.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"235 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758131","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Huaying Liu, Qisong Xing, Chenyu Zhu, Qineng Wang, Keding Lu, Song Guo, Zhijun Wu, Min Hu, Shao-Meng Li, Maosheng Yao
Endotoxin (lipopolysaccharide, LPS), widely distributed in the atmospheric environment with strong immunogenicity, is an important biological component of ambient particulate matter. However, whether LPS participates in atmospheric chemistry and how its biological health impacts change with the relevant processes are poorly understood. In this study, we employed the rat model to investigate the impact of ozone oxidation on the biological toxicity of LPS and used Fourier transform infrared spectroscopy and high-resolution electrospray mass spectrometry to study the underlying reaction mechanisms. The results show that the LPS can be oxidized by ozone and the resulting reactant greatly enhanced inflammatory anemia with a 177% capacity increase despite a minor influence on its immunogenicity. In contrast to the control, rats exposed to oxidized LPS were observed to release characteristic exhaled biomarkers, indicating that the formed reactant indeed altered the biological effects of LPS. Mechanistic investigation reveals that ozone oxidation of the hydroxyl group in the key toxic part of LPS, kdo2-lipid A, can cause dysregulation of iron homeostasis in rats, which is the mechanism of oxidized LPS-enhanced anemia. Unfortunately, these chemical structure changes and the resulting health impacts cannot be detected by the conventional LPS analysis method. This study highlights the changes in the toxicity of LPS and its health impacts when oxidized by ozone and the need to broadly consider the involvement of bioaerosol in atmospheric chemistry.
{"title":"Exposure to Endotoxin Oxidized by Atmospheric Ozone Greatly Enhances Anemia","authors":"Huaying Liu, Qisong Xing, Chenyu Zhu, Qineng Wang, Keding Lu, Song Guo, Zhijun Wu, Min Hu, Shao-Meng Li, Maosheng Yao","doi":"10.1021/acs.est.4c14589","DOIUrl":"https://doi.org/10.1021/acs.est.4c14589","url":null,"abstract":"Endotoxin (lipopolysaccharide, LPS), widely distributed in the atmospheric environment with strong immunogenicity, is an important biological component of ambient particulate matter. However, whether LPS participates in atmospheric chemistry and how its biological health impacts change with the relevant processes are poorly understood. In this study, we employed the rat model to investigate the impact of ozone oxidation on the biological toxicity of LPS and used Fourier transform infrared spectroscopy and high-resolution electrospray mass spectrometry to study the underlying reaction mechanisms. The results show that the LPS can be oxidized by ozone and the resulting reactant greatly enhanced inflammatory anemia with a 177% capacity increase despite a minor influence on its immunogenicity. In contrast to the control, rats exposed to oxidized LPS were observed to release characteristic exhaled biomarkers, indicating that the formed reactant indeed altered the biological effects of LPS. Mechanistic investigation reveals that ozone oxidation of the hydroxyl group in the key toxic part of LPS, kdo<sub>2</sub>-lipid A, can cause dysregulation of iron homeostasis in rats, which is the mechanism of oxidized LPS-enhanced anemia. Unfortunately, these chemical structure changes and the resulting health impacts cannot be detected by the conventional LPS analysis method. This study highlights the changes in the toxicity of LPS and its health impacts when oxidized by ozone and the need to broadly consider the involvement of bioaerosol in atmospheric chemistry.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"16 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758127","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Wenting Yuan, Lifang Zhang, Wangchao Zhao, Bo Yang, Xiaoqiao Jiao, Li Zhou, Huizhong Shen, Jianhuai Ye, Lei Zhu, Tzung-May Fu, Xin Yang, Chen Wang
Nitrous acid (HONO) and ozone (O3) are two important indoor pollutants that affect the indoor oxidation capacity. Previous field studies have observed an inverse correlation between these two pollutants indoors, but the specific mechanism remains unclear. Given the semivolatile behavior of HONO, a possible mechanism is its multiphase reaction with ozone. In this study, we measured ozone uptake on surface HONO/NO2– under environmentally relevant conditions in a flow tube. The ozone deposition velocities (vd = 0.002 ± 0.001–0.3 ± 0.005 cm s–1) and uptake coefficients (γ = (0.2 ± 0.1) × 10–6–(2.0 ± 0.2) × 10–4) depend on reactant concentrations, relative humidity, and reaction time but are less affected by illumination. The lifetimes of gaseous HONO and ozone are approximately 10 min due to this multiphase reaction under indoor conditions, which is a significant sink for HONO and O3 as compared to those of other indoor reactions and air exchange. This study for the first time revealed the previously overlooked vital role of the reaction of surface HONO/NO2– with O3 in affecting both indoor HONO and O3 and has significance for understanding the multiphase chemistry of HONO and O3, with implications for outdoor surfaces and model studies to better constrain HONO sinks.
{"title":"Multiphase Reaction of Ozone with HONO/NO2– on Surfaces: Effects on Indoor HONO and Ozone","authors":"Wenting Yuan, Lifang Zhang, Wangchao Zhao, Bo Yang, Xiaoqiao Jiao, Li Zhou, Huizhong Shen, Jianhuai Ye, Lei Zhu, Tzung-May Fu, Xin Yang, Chen Wang","doi":"10.1021/acs.est.5c01450","DOIUrl":"https://doi.org/10.1021/acs.est.5c01450","url":null,"abstract":"Nitrous acid (HONO) and ozone (O<sub>3</sub>) are two important indoor pollutants that affect the indoor oxidation capacity. Previous field studies have observed an inverse correlation between these two pollutants indoors, but the specific mechanism remains unclear. Given the semivolatile behavior of HONO, a possible mechanism is its multiphase reaction with ozone. In this study, we measured ozone uptake on surface HONO/NO<sub>2</sub><sup>–</sup> under environmentally relevant conditions in a flow tube. The ozone deposition velocities (<i>v</i><sub>d</sub> = 0.002 ± 0.001–0.3 ± 0.005 cm s<sup>–1</sup>) and uptake coefficients (γ = (0.2 ± 0.1) × 10<sup>–6</sup>–(2.0 ± 0.2) × 10<sup>–4</sup>) depend on reactant concentrations, relative humidity, and reaction time but are less affected by illumination. The lifetimes of gaseous HONO and ozone are approximately 10 min due to this multiphase reaction under indoor conditions, which is a significant sink for HONO and O<sub>3</sub> as compared to those of other indoor reactions and air exchange. This study for the first time revealed the previously overlooked vital role of the reaction of surface HONO/NO<sub>2</sub><sup>–</sup> with O<sub>3</sub> in affecting both indoor HONO and O<sub>3</sub> and has significance for understanding the multiphase chemistry of HONO and O<sub>3</sub>, with implications for outdoor surfaces and model studies to better constrain HONO sinks.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"183 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758128","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The accumulation of microplastics (MPs) in estuarine regions and their ecological consequences have become global environmental concerns. Estuarine sediments function as major sinks for MPs and hotspots for critical biogeochemical processes, which are significantly influenced by benthic bioturbation. However, the impacts of MPs on the behavior of highly mobile benthic organisms and the ecological effects of bioturbation activities remain poorly understood. This study utilized laboratory simulation experiments, AI-based behavioral tracking, and metagenomic sequencing to systematically examine the effects of sand crab bioturbation on MPs migration, sediment physicochemical properties and sulfur cycling processes. Results demonstrated that sand crab bioturbation substantially enhanced the vertical migration of MPs, with fluxes to surface layers and the overlying water increasing by 27-fold compared to undisturbed conditions. Exposure to PE-MPs reduced sand crabs’ surface foraging intensity and induced behavioral abnormalities. The crabs actively avoided MPs, exhibiting a preference for burrowing and residing in deeper sediment layers. This behavioral shift significantly altered microbial community distributions, with an increase of Pseudomonadota abundance and a decline of sulfate-reducing bacteria Thermodesulfobacteriota abundance. Furthermore, bioturbation accelerated sulfate oxidation in deeper sediments while inhibited dissimilatory sulfate reduction. This study is the first to identify the role of bioturbation in promoting the upward migration of MPs in sediments. Altered sand crab bioturbation will impact sediment biogeochemistry, estuarine function, and coastal resilience.
{"title":"Impact of Microplastic Exposure on Sand Crab Scopimera globosa Behavior: Implications for Microplastic Transport and Sulfur Cycling through Bioturbation","authors":"Chaofan Sun, Hui Liu, Jia Teng, Weiwei Feng, Dongyu Wang, Xiaodan Wang, Jianmin Zhao, Qing Wang","doi":"10.1021/acs.est.5c01192","DOIUrl":"https://doi.org/10.1021/acs.est.5c01192","url":null,"abstract":"The accumulation of microplastics (MPs) in estuarine regions and their ecological consequences have become global environmental concerns. Estuarine sediments function as major sinks for MPs and hotspots for critical biogeochemical processes, which are significantly influenced by benthic bioturbation. However, the impacts of MPs on the behavior of highly mobile benthic organisms and the ecological effects of bioturbation activities remain poorly understood. This study utilized laboratory simulation experiments, AI-based behavioral tracking, and metagenomic sequencing to systematically examine the effects of sand crab bioturbation on MPs migration, sediment physicochemical properties and sulfur cycling processes. Results demonstrated that sand crab bioturbation substantially enhanced the vertical migration of MPs, with fluxes to surface layers and the overlying water increasing by 27-fold compared to undisturbed conditions. Exposure to PE-MPs reduced sand crabs’ surface foraging intensity and induced behavioral abnormalities. The crabs actively avoided MPs, exhibiting a preference for burrowing and residing in deeper sediment layers. This behavioral shift significantly altered microbial community distributions, with an increase of <i>Pseudomonadota</i> abundance and a decline of sulfate-reducing bacteria <i>Thermodesulfobacteriota</i> abundance. Furthermore, bioturbation accelerated sulfate oxidation in deeper sediments while inhibited dissimilatory sulfate reduction. This study is the first to identify the role of bioturbation in promoting the upward migration of MPs in sediments. Altered sand crab bioturbation will impact sediment biogeochemistry, estuarine function, and coastal resilience.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"22 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143745147","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-01Epub Date: 2025-03-10DOI: 10.1021/acs.est.4c13266
Lin Luo, Chang Gao, Yi-Jun Fan, Ting Zhuang, Yuanyuan Li, Chang-An Li, Jia Lv, Zhong-Wang Hu, Lin Tao, Robert Gibson, Hua Wang, De-Xiang Xu, Yichao Huang
Bisphenol analogues have been shown to have similar estrogenic activity to that of BPA and may affect fetal development. However, no human studies have examined the effects of perinatal exposure to emerging bisphenol alternatives [bisphenol G, bisphenol M, and bisphenol BP (BPBP)] on small for gestational age (SGA) and how placental function may mediate the relationship. Here, 13 urinary bisphenol analogues were detected in 1054 contemporary pregnant women, and BPA was still the most dominant congener. Logistic regressions identified BPA and its traditional alternatives [bisphenol B (BPB), bisphenol E (BPE), bisphenol Z, and bisphenol AP (BPAP)] as being associated with an elevated risk of SGA (all ORs > 1.80, P < 0.05). In contrast, the emerging substitutes, despite high occurrences, all showed much attenuated risk. Mixture effect models Bayesian kernel machine regression and quantile-based g-computation demonstrated that coexposure to bisphenols was strongly correlated with SGA risk (OR = 2.70, P < 0.001), with BPA and the conventional substitutes (BPB, BPE, and BPAP) as primary effect drivers, outweighing the effect from emerging substitutes. Finally, mediation analysis revealed that the placental function index estriol mediated the relationship between exposure and SGA, dominated by BPBP (25.4%). Our findings provide new epidemiological evidence that early BPA alternatives may pose a higher risk for offspring development than those emerging alternatives, potentially via mediation by compromised placental function. Future toxicity assessments and validation studies in other settings on these emerging bisphenols are needed.
{"title":"Perinatal Bisphenol Exposure and Small-for-Gestational-Age Neonates: The Evolving Effect of Replacements Then and Now.","authors":"Lin Luo, Chang Gao, Yi-Jun Fan, Ting Zhuang, Yuanyuan Li, Chang-An Li, Jia Lv, Zhong-Wang Hu, Lin Tao, Robert Gibson, Hua Wang, De-Xiang Xu, Yichao Huang","doi":"10.1021/acs.est.4c13266","DOIUrl":"10.1021/acs.est.4c13266","url":null,"abstract":"<p><p>Bisphenol analogues have been shown to have similar estrogenic activity to that of BPA and may affect fetal development. However, no human studies have examined the effects of perinatal exposure to emerging bisphenol alternatives [bisphenol G, bisphenol M, and bisphenol BP (BPBP)] on small for gestational age (SGA) and how placental function may mediate the relationship. Here, 13 urinary bisphenol analogues were detected in 1054 contemporary pregnant women, and BPA was still the most dominant congener. Logistic regressions identified BPA and its traditional alternatives [bisphenol B (BPB), bisphenol E (BPE), bisphenol Z, and bisphenol AP (BPAP)] as being associated with an elevated risk of SGA (all ORs > 1.80, <i>P</i> < 0.05). In contrast, the emerging substitutes, despite high occurrences, all showed much attenuated risk. Mixture effect models Bayesian kernel machine regression and quantile-based <i>g</i>-computation demonstrated that coexposure to bisphenols was strongly correlated with SGA risk (OR = 2.70, <i>P</i> < 0.001), with BPA and the conventional substitutes (BPB, BPE, and BPAP) as primary effect drivers, outweighing the effect from emerging substitutes. Finally, mediation analysis revealed that the placental function index estriol mediated the relationship between exposure and SGA, dominated by BPBP (25.4%). Our findings provide new epidemiological evidence that early BPA alternatives may pose a higher risk for offspring development than those emerging alternatives, potentially via mediation by compromised placental function. Future toxicity assessments and validation studies in other settings on these emerging bisphenols are needed.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":"5983-5993"},"PeriodicalIF":10.8,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143583808","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yuan Yu, Chi Ding, Hailong Tong, Nanqi Ren, Shijie You
Freeze desalination (FD) offers a promising solution for desalining industrial saline wastewater in cold regions. However, salt entrapment in the close-dendritic ice pore network is uncontrollable, which makes ice-salt separation a challenge. To address this issue, this study reported the electro-assisted crystallization (EAC) to realize the controllable FD, inspired by the ice purification during insulator flashover frequently observed in power transmission systems. The experiment performed at −20 °C demonstrated that EAC allowed ice crystallization with an open ice pore network, whose open-area percentage was increased from 25 to 41% as current density was raised from 10 to 30 mA cm–2. The EAC could achieve 89.3% desalination efficiency from 35 g L–1 saltwater at 30 mA cm–2, the value being four times that obtained for direct FD. Based on the principle of physical field synergy, the spontaneous salt release and controllable FD were likely the results of electro-heat synergy between Joule heating and dipole polarization effects. This study not only provides a novel pathway for controllable ice-salt separation inspired by flashover phenomenon but also suggests a potential technology for desalination treatment of water or wastewater in cold regions.
{"title":"Flashover-Inspired Electro-Assisted Crystallization for Controllable Freeze Desalination","authors":"Yuan Yu, Chi Ding, Hailong Tong, Nanqi Ren, Shijie You","doi":"10.1021/acs.est.4c14381","DOIUrl":"https://doi.org/10.1021/acs.est.4c14381","url":null,"abstract":"Freeze desalination (FD) offers a promising solution for desalining industrial saline wastewater in cold regions. However, salt entrapment in the close-dendritic ice pore network is uncontrollable, which makes ice-salt separation a challenge. To address this issue, this study reported the electro-assisted crystallization (EAC) to realize the controllable FD, inspired by the ice purification during insulator flashover frequently observed in power transmission systems. The experiment performed at −20 °C demonstrated that EAC allowed ice crystallization with an open ice pore network, whose open-area percentage was increased from 25 to 41% as current density was raised from 10 to 30 mA cm<sup>–2</sup>. The EAC could achieve 89.3% desalination efficiency from 35 g L<sup>–1</sup> saltwater at 30 mA cm<sup>–2</sup>, the value being four times that obtained for direct FD. Based on the principle of physical field synergy, the spontaneous salt release and controllable FD were likely the results of electro-heat synergy between Joule heating and dipole polarization effects. This study not only provides a novel pathway for controllable ice-salt separation inspired by flashover phenomenon but also suggests a potential technology for desalination treatment of water or wastewater in cold regions.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"22 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758135","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Emily M. Hammermeister, Stathys Papadimitriou, Martin Arundell, Jake Ludgate, Allison Schaap, Matthew C. Mowlem, Sara E. Fowell, Edward Chaney, Socratis Loucaides
The development of marine autonomous platforms has improved our capability to gather ocean observations at fine spatial scales and high temporal frequency, which can be used to better measure, characterize, and model ocean carbon. As part of the OCEANIDS program, novel carbonate sensors were integrated into the Autosub Long-Range (ALR) autonomous underwater vehicle (AUV) and deployed in the Celtic Sea. Autonomous Lab-On-Chip (LOC) sensors measured pH and total alkalinity (TA) while onboard the ALR. Using interpolation, the ALR-sensor data set is compared against CTD co-samples. The average differences between the LOC sensor and co-sample pH range from −0.011 to −0.015. The TA sensor data agrees with co-samples within 1–2 μmol kg–1 on average. Biogeochemical water properties differing between CTD and ALR observations reveal correlations to carbonate parameter variations. The LOC sensors enabled the characterization of the marine carbonate system from autonomous subsurface measurements for the first time. Sensor pH and TA data were used to calculate dissolved inorganic carbon (DIC), partial pressure of CO2 (pCO2), and aragonite saturation state (ΩAr) and are compared with CTD co-samples with mean residuals of 4–7 μmol kg–1, 10–17 μatm, and −0.03 to −0.06, respectively. Future perspectives on sensor deployment and analysis are discussed.
{"title":"New Capability in Autonomous Ocean Carbon Observations Using the Autosub Long-Range AUV Equipped with Novel pH and Total Alkalinity Sensors","authors":"Emily M. Hammermeister, Stathys Papadimitriou, Martin Arundell, Jake Ludgate, Allison Schaap, Matthew C. Mowlem, Sara E. Fowell, Edward Chaney, Socratis Loucaides","doi":"10.1021/acs.est.4c10139","DOIUrl":"https://doi.org/10.1021/acs.est.4c10139","url":null,"abstract":"The development of marine autonomous platforms has improved our capability to gather ocean observations at fine spatial scales and high temporal frequency, which can be used to better measure, characterize, and model ocean carbon. As part of the OCEANIDS program, novel carbonate sensors were integrated into the Autosub Long-Range (ALR) autonomous underwater vehicle (AUV) and deployed in the Celtic Sea. Autonomous Lab-On-Chip (LOC) sensors measured pH and total alkalinity (TA) while onboard the ALR. Using interpolation, the ALR-sensor data set is compared against CTD co-samples. The average differences between the LOC sensor and co-sample pH range from −0.011 to −0.015. The TA sensor data agrees with co-samples within 1–2 μmol kg<sup>–1</sup> on average. Biogeochemical water properties differing between CTD and ALR observations reveal correlations to carbonate parameter variations. The LOC sensors enabled the characterization of the marine carbonate system from autonomous subsurface measurements for the first time. Sensor pH and TA data were used to calculate dissolved inorganic carbon (DIC), partial pressure of CO<sub>2</sub> (pCO<sub>2</sub>), and aragonite saturation state (Ω<sub>Ar</sub>) and are compared with CTD co-samples with mean residuals of 4–7 μmol kg<sup>–1</sup>, 10–17 μatm, and −0.03 to −0.06, respectively. Future perspectives on sensor deployment and analysis are discussed.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"32 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758132","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
How to scientifically and efficiently quantify the impact and hazards of volatile organic compounds (VOCs) pollution and volatilization from complex groundwater systems on surface air environments is a critical environmental issue. This paper employed an integrated modeling approach, incorporating numerical simulations, statistical analyses, and machine learning to address this issue. We comprehensively accounted for the different driving mechanisms, along with the various migration and transformation processes of groundwater VOCs. This investigation identified 11 key factors influencing surface pollutant flux. The data-enhanced statistical surrogate models and sampling-fusion-based support vector machine (SVM) surrogate models were established for appropriate generic modeling applications in which the high computation burden and difficulty could be avoided of the complicated numerical modeling. Those models would enable accurate prediction of surface fluxes and reliable classification of environmental risks. Notably, the pollutant fluxes through the soil–air interface over a short period could be sufficient to cause slow-airflow space air concentrations to exceed acceptable levels. Particularly, the established generic statistical surrogate models and SVM surrogate models have significant implications in efficiently and rapidly assessing the VOCs surface fluxes and environmental risk with meaningful quantified uncertainties for specific site conditions.
{"title":"Machine Learning-Enhanced Prediction for Soil-to-Air VOC Emission and Environmental Impact Pertaining Contaminated Fractured Aquifers","authors":"Tianyu He, Cixiao Qu, Mingyu Wang","doi":"10.1021/acs.est.4c09065","DOIUrl":"https://doi.org/10.1021/acs.est.4c09065","url":null,"abstract":"How to scientifically and efficiently quantify the impact and hazards of volatile organic compounds (VOCs) pollution and volatilization from complex groundwater systems on surface air environments is a critical environmental issue. This paper employed an integrated modeling approach, incorporating numerical simulations, statistical analyses, and machine learning to address this issue. We comprehensively accounted for the different driving mechanisms, along with the various migration and transformation processes of groundwater VOCs. This investigation identified 11 key factors influencing surface pollutant flux. The data-enhanced statistical surrogate models and sampling-fusion-based support vector machine (SVM) surrogate models were established for appropriate generic modeling applications in which the high computation burden and difficulty could be avoided of the complicated numerical modeling. Those models would enable accurate prediction of surface fluxes and reliable classification of environmental risks. Notably, the pollutant fluxes through the soil–air interface over a short period could be sufficient to cause slow-airflow space air concentrations to exceed acceptable levels. Particularly, the established generic statistical surrogate models and SVM surrogate models have significant implications in efficiently and rapidly assessing the VOCs surface fluxes and environmental risk with meaningful quantified uncertainties for specific site conditions.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"22 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143745144","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Alper James Alcaraz, Sydney Murray, Phillip Ankley, Bradley Park, Katherine Raes, Shakya Kurukulasuriya, Doug Crump, Niladri Basu, Markus Brinkmann, Markus Hecker, Natacha Hogan
New approach methods (NAMs) are urgently needed to address the significant ethical and economic concerns associated with live animal testing as well as the low throughput associated with current toxicity testing frameworks. NAMs such as rapid mechanistic early-life-stage fish assays are promising alternatives to current hazard assessment approaches, as they can be used to derive toxicity thresholds and guide decision-makers on identifying or prioritizing chemicals of concern. This study aimed to derive benchmark concentrations from RNaseq data (transcriptomic points-of-departure; tPOD) from a short-term exposure study with early life stages of rainbow trout (RBT; Oncorhynchus mykiss) using benzo[a]pyrene (B[a]P) as the model compound. tPODs were then calibrated with higher organizational-level responses observed during an extended 28 day exposure period. RBT were exposed from 1 to 28 days post-hatch (dph) to 0.079, 0.35, 1.5, 7.4, and 29 μg/L (28 d time weighted average measured) B[a]P, as well as 0.05% dimethyl sulfoxide and water only controls. Benchmark concentration analysis of transcriptomic responses at 4 dph, based on the most sensitive transcriptomic features, yielded tPODs between 0.028 and 0.47 μg/L B[a]P. At 28 dph, Cyp1a1 exhibited significantly increased catalytic activity, with biochemical POD, bPODEROD,28dph of 0.599 μg/L B[a]P, while morphometric analysis showed significant growth inhibition in terms of length, with apical POD, aPODlength,28dph of 1.77 μg/L B[a]P, with a notable decreasing trend in body weight. A toxicity pathway model constructed from genes and apical end points exhibiting concentration-dependent responses provided further evidence supporting the utility of tPODs from short-term RBT early-life-stage assay to support chemical risk assessment to guide decision-makers in chemical testing prioritization.
{"title":"Transcriptomics Points-of-Departure (tPODs) to Support Hazard Assessment of Benzo[a]pyrene in Early-Life-Stage Rainbow Trout","authors":"Alper James Alcaraz, Sydney Murray, Phillip Ankley, Bradley Park, Katherine Raes, Shakya Kurukulasuriya, Doug Crump, Niladri Basu, Markus Brinkmann, Markus Hecker, Natacha Hogan","doi":"10.1021/acs.est.4c11870","DOIUrl":"https://doi.org/10.1021/acs.est.4c11870","url":null,"abstract":"New approach methods (NAMs) are urgently needed to address the significant ethical and economic concerns associated with live animal testing as well as the low throughput associated with current toxicity testing frameworks. NAMs such as rapid mechanistic early-life-stage fish assays are promising alternatives to current hazard assessment approaches, as they can be used to derive toxicity thresholds and guide decision-makers on identifying or prioritizing chemicals of concern. This study aimed to derive benchmark concentrations from RNaseq data (transcriptomic points-of-departure; tPOD) from a short-term exposure study with early life stages of rainbow trout (RBT; <i>Oncorhynchus mykiss</i>) using benzo[<i>a</i>]pyrene (B[<i>a</i>]P) as the model compound. tPODs were then calibrated with higher organizational-level responses observed during an extended 28 day exposure period. RBT were exposed from 1 to 28 days post-hatch (dph) to 0.079, 0.35, 1.5, 7.4, and 29 μg/L (28 d time weighted average measured) B[<i>a</i>]P, as well as 0.05% dimethyl sulfoxide and water only controls. Benchmark concentration analysis of transcriptomic responses at 4 dph, based on the most sensitive transcriptomic features, yielded tPODs between 0.028 and 0.47 μg/L B[<i>a</i>]P. At 28 dph, Cyp1a1 exhibited significantly increased catalytic activity, with biochemical POD, bPOD<sub>EROD,28dph</sub> of 0.599 μg/L B[<i>a</i>]P, while morphometric analysis showed significant growth inhibition in terms of length, with apical POD, aPOD<sub>length,28dph</sub> of 1.77 μg/L B[<i>a</i>]P, with a notable decreasing trend in body weight. A toxicity pathway model constructed from genes and apical end points exhibiting concentration-dependent responses provided further evidence supporting the utility of tPODs from short-term RBT early-life-stage assay to support chemical risk assessment to guide decision-makers in chemical testing prioritization.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"33 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143745146","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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